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用锰矿石对水中苯胺进行催化臭氧化

Catalytic ozonation of phenylamine in water with a manganese ore.

作者信息

Feng Yingming, Li Xiaobing

机构信息

National Engineering Research Center of Coal Preparation and Purification, China University of Mining and Technology No. 1 Daxue Road Xuzhou Jiangsu 221116 PR China

China Kunlun Contracting & Engineering Corporation Beijing 100013 PR China.

出版信息

RSC Adv. 2020 Oct 1;10(59):36192-36200. doi: 10.1039/d0ra05464j. eCollection 2020 Sep 28.

Abstract

Recalcitrant pollutants, which form surface complexes with surface metal sites of the catalyst, are difficult to remove by catalytic ozonation in water. Phenylamine (PA), one of the refractory pollutants, was degraded by ozone catalysis with manganese ore in this paper. And the effectiveness and the mechanism of catalytic ozonation with manganese ore for the degradation of PA in water were studied. After the BET test, the specific surface area of the raw and calcined manganese ore was 27.65 m g and 33.49 m g, respectively. The effects of solution pH, catalyst dose and reaction time on the degradation of PA were evaluated. Results showed that the catalytic potential of calcined manganese ore was better than that of raw manganese ore and ozonation alone in the degradation of PA. It revealed that the increase of hydroxyl radicals generated on the surface of the catalyst or in the solution improved PA degradation. Oxidation of free radicals was the main mechanism of PA degradation in the catalytic ozonation process, occurring with a pseudo-first-order reaction rate at a constant of 0.0993 min (CMP) under the pH of 7.20 and catalyst dose of 3 g L. Also, an activation energy of 20.4 kJ mol for PA oxidation over CMP in the presence of O was estimated.

摘要

顽固性污染物会与催化剂的表面金属位点形成表面络合物,因此难以通过水中的催化臭氧化去除。苯胺(PA)是难降解污染物之一,本文研究了用锰矿进行臭氧催化降解PA的效果及机理。通过BET测试可知,原锰矿和煅烧后锰矿的比表面积分别为27.65 m²/g和33.49 m²/g。评估了溶液pH值、催化剂用量和反应时间对PA降解的影响。结果表明,在PA降解过程中,煅烧锰矿的催化潜力优于原锰矿和单独臭氧化。这表明催化剂表面或溶液中产生的羟基自由基增加促进了PA的降解。自由基氧化是催化臭氧化过程中PA降解的主要机制,在pH值为7.20、催化剂用量为3 g/L的条件下,以0.0993 min⁻¹(CMP)的准一级反应速率发生。此外,估算了在O₃存在下,PA在CMP上氧化的活化能为20.4 kJ/mol。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5404/9056967/6a7dd3b3abd8/d0ra05464j-f1.jpg

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